CN111511457A - Multilayer three-way catalytic converter - Google Patents

Multilayer three-way catalytic converter Download PDF

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Publication number
CN111511457A
CN111511457A CN201880081997.4A CN201880081997A CN111511457A CN 111511457 A CN111511457 A CN 111511457A CN 201880081997 A CN201880081997 A CN 201880081997A CN 111511457 A CN111511457 A CN 111511457A
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cerium
zirconium
rare earth
oxide
earth metal
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J·舍恩哈贝尔
M·罗施
J-M·里希特
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Umicore Corp And Lianghe Co
Umicore AG and Co KG
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Umicore Corp And Lianghe Co
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    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
    • B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
    • B01D53/9445—Simultaneously removing carbon monoxide, hydrocarbons or nitrogen oxides making use of three-way catalysts [TWC] or four-way-catalysts [FWC]
    • B01D53/945—Simultaneously removing carbon monoxide, hydrocarbons or nitrogen oxides making use of three-way catalysts [TWC] or four-way-catalysts [FWC] characterised by a specific catalyst
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    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
    • B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
    • B01D53/9459—Removing one or more of nitrogen oxides, carbon monoxide, or hydrocarbons by multiple successive catalytic functions; systems with more than one different function, e.g. zone coated catalysts
    • B01D53/9463—Removing one or more of nitrogen oxides, carbon monoxide, or hydrocarbons by multiple successive catalytic functions; systems with more than one different function, e.g. zone coated catalysts with catalysts positioned on one brick
    • B01D53/9468—Removing one or more of nitrogen oxides, carbon monoxide, or hydrocarbons by multiple successive catalytic functions; systems with more than one different function, e.g. zone coated catalysts with catalysts positioned on one brick in different layers
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    • B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
    • B01J21/06—Silicon, titanium, zirconium or hafnium; Oxides or hydroxides thereof
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    • B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
    • B01J35/56—Foraminous structures having flow-through passages or channels, e.g. grids or three-dimensional monoliths
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/02—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust
    • F01N3/021—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters
    • F01N3/033—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters in combination with other devices
    • F01N3/035—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters in combination with other devices with catalytic reactors, e.g. catalysed diesel particulate filters
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    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
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    • F01N3/101—Three-way catalysts
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    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
    • F01N3/24—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by constructional aspects of converting apparatus
    • F01N3/28—Construction of catalytic reactors
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    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
    • F01N3/24—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by constructional aspects of converting apparatus
    • F01N3/28—Construction of catalytic reactors
    • F01N3/2803—Construction of catalytic reactors characterised by structure, by material or by manufacturing of catalyst support
    • F01N3/2825—Ceramics
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Abstract

The invention relates to a three-way catalytic converter which is particularly suitable for removing carbon monoxide, hydrocarbons and nitrogen oxides from the exhaust gas of internal combustion engines which are operated with a stoichiometric air-fuel mixture. The three-way catalytic converter is characterized in that it has a high oxygen storage capacity after aging and consists of at least two catalytically active layers.

Description

Multilayer three-way catalytic converter
The invention relates to a three-way catalytic converter which is particularly suitable for removing carbon monoxide, hydrocarbons and nitrogen oxides from the exhaust gas of internal combustion engines which are operated with a stoichiometric air-fuel mixture. Characterized in that the three-way catalytic converter has a high oxygen storage capacity after ageing and consists of at least two catalytically active layers.
Exhaust gases from internal combustion engines operated with a stoichiometric air-fuel mixture (i.e. gasoline or natural gas fueled engines) are cleaned in a conventional process by means of a three-way catalytic converter. Such catalytic converters are capable of simultaneously converting the three main gaseous pollutants of the engine, namely hydrocarbons, carbon monoxide and nitrogen oxides, into harmless components. Stoichiometrically, on average, the amount of air used to combust the fuel present in the cylinder is the same as the amount of air required for complete combustion. Setting the combustion air ratio lambda (A/F ratio; air/fuel ratio) to the air mass m that can be actually obtained for combustionLActual compared to stoichiometric air mass mLAnd (2) stoichiometric:
Figure BDA0002545797090000011
if λ <1 (e.g., 0.9), then "air deficit" is indicated, i.e., a rich exhaust gas mixture; λ >1 (e.g., 1.1) represents "air excess," i.e., a lean-burn exhaust gas mixture. The expression λ 1.1 means that 10% more air is present than is required for the stoichiometric reaction.
Usually, platinum group metals are used as catalytically active materials, in particular platinum, palladium and rhodium, which are present, for example, as support materials on gamma alumina. In addition, the three-way catalytic converter contains an oxygen storage material, such as a cerium/zirconium mixed oxide. In the latter case, cerium oxide (a rare earth oxide) constitutes the basic component for oxygen storage. In addition to zirconia and ceria, these materials may also contain additional components, such as additional rare earth metal oxides or alkaline earth metal oxides. The oxygen storage material is activated by application of a catalytically active material such as a platinum group metal and therefore also serves as a support material for the platinum group metal.
The components of the three-way catalytic converter may be present in a single coating on an inert catalyst support. Such catalytic converters are characterized by lower coating costs compared to multilayer catalytic converters.
EP1541220B1 describes a single-layer three-way catalytic converter in which palladium and rhodium are present predominantly in unalloyed form.
EP1974810B1 describes a single-layer three-way catalytic converter in which a first cerium/zirconium mixed oxide is activated by rhodium and a second cerium/zirconium mixed oxide is activated by palladium, the zirconia content of the first cerium/zirconium mixed oxide being higher than that of the second cerium/zirconium mixed oxide.
EP2948653a1 describes a single-layer three-way catalytic converter in which the temperature-resistant metal oxide and optionally a first cerium/zirconium mixed oxide is activated by rhodium and a second cerium/zirconium mixed oxide is activated by palladium, the proportion of cerium/zirconium mixed oxide in the layer being equal to or greater than the proportion of temperature-resistant metal oxide in the layer.
However, often double-layer catalysts are used, which facilitate the separation of the different catalytic processes and thus achieve an optimal coordination of the catalytic effects in the two layers. This often results in a multilayer catalytic converter having higher aging stability than a single layer catalytic converter. Catalytic converters of the latter type are disclosed, for example, in WO9535152a1, WO2008000449a2, EP0885650a2, EP1046423a2, EP1726359a1 and EP1974809a 1.
EP1974809a1 discloses a two-layer three-way catalytic converter comprising cerium/zirconium mixed oxide in both layers, wherein the cerium/zirconium mixed oxide in the top layer has a correspondingly higher proportion of zirconium than in the bottom layer.
EP1726359a1 describes a two-layer three-way catalyst which comprises a cerium/zirconium/lanthanum/neodymium mixed oxide with a zirconium content of more than 80 mol% in both layers, wherein the zirconium proportion of the cerium/zirconium/lanthanum/neodymium mixed oxide in the top layer can be correspondingly higher than in the bottom layer.
WO2008000449a2 also discloses a two-layer catalytic converter comprising cerium/zirconium mixed oxide in both layers, and in which the mixed oxide in the top layer again has a higher proportion of zirconium. To some extent, the cerium/zirconium mixed oxide can also be replaced by a cerium/zirconium/lanthanum/neodymium mixed oxide or a cerium/zirconium/lanthanum/yttrium mixed oxide.
Three-way catalytic converters known in the prior art have a certain oxygen storage capacity after aging. Known compositions of three-way catalytic converters are described, for example, in EP3045226a1 and EP3247493a 1. In modern vehicles with direct gasoline injection, these exhibit very low emissions. Surprisingly, it has been found that in vehicles with intake manifold injection, three-way catalytic converters have particularly low emissions, which are characterized by a high static oxygen storage capacity.
The present invention relates to a three-way catalytic converter with increased oxygen storage capacity and improved emissions, in particular in a vehicle with intake manifold injection, comprising two layers on an inert catalyst support, wherein
Layer A comprises at least one activated alumina, one platinum group metal and at least two different cerium/zirconium/rare earth mixed oxides, and
layer B applied to layer a comprises at least one activated alumina, one platinum group metal and at least one cerium/zirconium/rare earth metal mixed oxide.
Surprisingly, it has been found that the combination of different cerium/zirconium/rare earth metal mixed oxides in one coating layer can greatly increase the conversion of gaseous pollutants after hard aging.
If in the context of the present invention a coating on a wall is mentioned, this means that only a small part of at most 20 wt.%, more preferably at most 15 wt.%, very particularly preferably at most 10 wt.%, most preferably at most 5 wt.% of the coating is present in the wall of the flow substrate, this can be determined by graphic analysis of SEM cross-sectional images.
Coating B is at least partially on coating a. In a preferred embodiment, coating B covers at least 50%, preferably at least 70%, very preferably 100% of coating a.
Coating a has catalytic activity, especially at operating temperatures of 250 ℃ to 1100 ℃. It generally comprises one or more noble metals immobilized on one or more support materials and two oxygen storage components which differ from one another. The oxygen storage component is different with respect to at least one of the components contained. The same components of the oxygen storage material may be present in the same or different amounts.
Coating B has catalytic activity, especially at operating temperatures of 250 ℃ to 1100 ℃. It generally comprises one or more noble metals immobilized on one or more support materials and at least one oxygen storage component.
Cerium/zirconium/rare earth metal mixed oxides are suitable as oxygen storage components. Within the meaning of the present invention, the term "cerium/zirconium/rare earth metal mixed oxide" does not include physical mixtures of cerium oxide, zirconium oxide and rare earth oxides. In contrast, a "cerium/zirconium/rare earth metal mixed oxide" is characterized by a substantially uniform three-dimensional crystal structure that is ideally free of phases of pure ceria, zirconia, or rare earth oxides. Depending on the manufacturing process, however, it is possible to produce incompletely homogeneous products with a homogeneity of > 80% by weight, which can generally be used without disadvantages. In all other aspects, the term "rare earth metal" or "rare earth metal oxide" within the meaning of the present invention does not include cerium or cerium oxide.
Lanthanum oxide, yttrium oxide, praseodymium oxide, neodymium oxide and/or samarium oxide can be considered, for example, as rare earth oxides in cerium/zirconium/rare earth mixed oxides.
Lanthanum oxide, yttrium oxide and/or praseodymium oxide are preferred, and lanthanum oxide and yttrium oxide, yttrium oxide and praseodymium oxide and lanthanum oxide and praseodymium oxide are very particularly preferred.
In an embodiment of the present invention, the oxygen storage component preferably does not contain neodymium oxide.
In an embodiment of the invention, the weight ratio of aluminum oxide to the sum of the two cerium/zirconium/rare earth metal mixed oxides in coating a is in the range from 10:90 to 60:40, preferably in the range from 20:80 to 50:50, particularly preferably in the range from 25:75 to 35: 65.
In a preferred embodiment, the coating a and/or B comprises lanthanum-stabilized alumina in an amount of in each case from 10 to 60% by weight, preferably from 20 to 50% by weight, particularly preferably from 25 to 35% by weight, and in each case from 40 to 90% by weight, preferably from 50 to 80% by weight, particularly preferably from 65 to 75% by weight, of oxygen storage component, based on the sum of the weights of alumina and oxygen storage component in the coating.
In a preferred embodiment, the proportion of cerium/zirconium/rare earth metal mixed oxide in the layer a is greater than the proportion of cerium/zirconium/rare earth metal mixed oxide in the layer B, in each case in% by weight and based on the total weight of the respective layer. In an embodiment, the coating a comprises two oxygen storage components which are different from one another, wherein the weight ratio of the first cerium/zirconium/rare earth metal mixed oxide to the second cerium/zirconium/rare earth metal mixed oxide is preferably in the range from 4:1 to 1:4, preferably in the range from 3:1 to 1:3, particularly preferably in the range from 2:1 to 1: 2.
According to the invention, the mass ratio of cerium oxide to zirconium oxide in the cerium/zirconium/rare earth metal mixed oxide of the layers a and/or B can vary within wide limits. This mass ratio is equal to, for example, 0.1 to 1.5, preferably 0.2 to 1.25 or 0.3 to 1.
In an embodiment of the invention, coating a comprises a first oxygen storage component and a second oxygen storage component, wherein the first oxygen storage component has a higher zirconia content than the second oxygen storage component. It is also preferred that the first oxygen storage component has a weight ratio of cerium oxide to zirconium oxide of 0.7 to 0.1 that is less than the weight ratio of cerium oxide to zirconium oxide of 0.5 to 1.5 that the second cerium/zirconium/rare earth metal mixed oxide has. Other more preferred embodiments include a first oxygen storage component having a ceria to zirconia weight ratio of 0.6 to 0.2 and a second oxygen storage component having a ceria to zirconia weight ratio of 0.6 to 1.2. Other most preferred embodiments include a first oxygen storage component having a ceria to zirconia weight ratio of 0.5 to 0.3 and a second oxygen storage component having a ceria to zirconia weight ratio of 0.7 to 1.0.
In a preferred embodiment, the three-way catalytic converter according to the invention is designed such that in the coating a the first cerium/zirconium/rare earth metal mixed oxide has a cerium oxide content of 10% to 40% by weight, based on the first cerium/zirconium/rare earth metal mixed oxide, more preferably 15% to 35% by weight, very particularly preferably 20% to 30% by weight, based on the first cerium/zirconium/rare earth metal mixed oxide.
In contrast, the zirconia content of the first cerium/zirconium/rare earth metal mixed oxide in coating a is 40% to 90% based on the weight of the first cerium/zirconium/rare earth metal mixed oxide. Advantageously, the zirconia content of the first cerium/zirconium/rare earth mixed oxide is between 50% and 75%, very preferably between 55% and 65%, based on the weight of the first cerium/zirconium/rare earth mixed oxide.
Likewise, the cerium oxide content of the second cerium/zirconium/rare earth metal mixed oxide in coating a should be predominantly 25% to 60%, based on the weight of the second cerium/zirconium/rare earth metal mixed oxide. More advantageously, in the second cerium/zirconium/rare earth mixed oxide, the cerium oxide content is between 30% and 55%, very preferably between 35% and 50%, based on the weight of the second cerium/zirconium/rare earth mixed oxide.
In another preferred embodiment, the second cerium/zirconium/rare earth metal mixed oxide in coating a has a zirconium oxide content of 20% to 70% based on the weight of the second cerium/zirconium/rare earth metal mixed oxide. It is more preferred here that the second cerium/zirconium/rare earth metal mixed oxide has a zirconium oxide content of from 30 to 60%, very particularly preferably from 40 to 55%, based on the weight of the second cerium/zirconium/rare earth metal mixed oxide.
It is preferred according to the invention that the cerium/zirconium/rare earth metal mixed oxide of layer a and optionally the at least one cerium/zirconium/rare earth metal mixed oxide of layer B are each doped with lanthanum oxide, so that preferably the lanthanum oxide content is > 0% to 10% based on the weight of the cerium/zirconium/rare earth metal mixed oxide. Particularly advantageously, these lanthanum oxide-containing oxygen storage components have a lanthanum oxide to cerium oxide mass ratio of 0.05 to 0.5.
The first cerium/zirconium/rare earth metal mixed oxide in layer a is preferably doped with yttrium oxide in addition to lanthanum oxide. The preferred catalytic converter has a yttria content of the first cerium/zirconium/rare earth metal mixed oxide of from 2% to 25% based on the weight of the first cerium/zirconium/rare earth metal mixed oxide. More preferably, the yttrium content of the first cerium/zirconium/rare earth metal mixed oxide is between 4% and 20%, very preferably between 10% and 15%, based on the weight of the first cerium/zirconium/rare earth metal mixed oxide.
An embodiment in which the second cerium/zirconium/rare earth mixed oxide of layer a is doped not only with lanthanum oxide but also with other metal oxides from the group of rare earth oxides, preferably with praseodymium, is also advantageous. The content of the second rare earth metal in the second cerium/zirconium/rare earth metal mixed oxide may be between 2% and 15% based on the weight of the second cerium/zirconium/rare earth metal mixed oxide. More advantageously, the second cerium/zirconium/rare earth metal mixed oxide has a content of the second rare earth metal of from 3% to 10%, very preferably from 4% to 8%, based on the weight of the second cerium/zirconium/rare earth metal mixed oxide.
An embodiment in which the cerium/zirconium/rare earth metal mixed oxide of coating B is doped not only with lanthanum oxide but also with other metal oxides from the group of rare earth metal oxides, preferably with praseodymium oxide and/or yttrium oxide, is also advantageous. The content of rare earth metal in the cerium/zirconium/rare earth metal mixed oxide of coating B may be between 2% and 15% based on the weight of the cerium/zirconium/rare earth metal mixed oxide. More advantageously, the content of rare earth metal of the cerium/zirconium/rare earth metal mixed oxide is from 3% to 10%, very preferably from 4% to 8%, based on the weight of the cerium/zirconium/rare earth metal mixed oxide in the coating B.
In the coating layers a and/or B, the praseodymium content of the second oxygen storage component is specifically 2 to 10% by weight, based on the weight of the respective oxygen storage component. The weight ratio of lanthanum oxide to praseodymium oxide is in particular from 0.1 to 2.0, preferably from 0.2 to 1.8, very preferably from 0.5 to 1.5.
In an embodiment of the invention, the zirconia content of the yttria-containing oxygen storage component is greater than the zirconia content of the praseodymia-containing oxygen storage component in the coating, in each case based on the respective oxygen storage component.
According to the invention, coating a and coating B contain noble metals as catalytically active elements. The layers a and B contain, independently of one another, platinum group metals, in particular platinum, palladium, rhodium or mixtures of at least two thereof, preferably at least two from these platinum group metals. In an embodiment of the invention, layer a comprises platinum, palladium or platinum and palladium and layer B comprises palladium, rhodium or palladium and rhodium.
Specifically, layer a comprises palladium and layer B comprises rhodium or palladium and rhodium.
The amount of noble metal used is generally from 0.1g/l to 15g/l, preferably from 0.15g/l to 10g/l, based on the volume of the ceramic honeycomb body. In a preferred embodiment, the noble metal is present in equal amounts on the alumina and the oxygen storage component.
As base material for the noble metal in the layers a and B, all materials known to the person skilled in the art can be considered for this purpose. Such materials are in particular metal oxides having a BET surface area of 30m2G to 250m2A/g, preferably of 100m2G to 200m2G (determined according to DIN 66132-latest version as of filing date). Cerium/zirconium/rare earth metal mixed oxides can be used as support materials for the platinum group metals in layer a and/or layer B. Furthermore, in layer a and/or layer B, they may also be supported in whole or in part on activated alumina.
Thus, in embodiments of the invention, layers A and B comprise activated alumina it is particularly preferred that the activated alumina is stabilised by doping, especially doping with lanthanum oxide a preferred activated alumina comprises from 1 to 6 wt%, especially from 3 to 4 wt% lanthanum oxide (L a)2O3)。
The term "activated alumina" is known to those skilled in the art. In particular, it describes a surface area of 100m2G to 200m2Gamma oxidation of/gAluminum. Activated alumina is often described in the literature and is commercially available.
The coating A and/or B generally comprises oxygen storage components in an amount of from 30g/l to 225g/l, preferably from 40g/l to 200g/l, particularly preferably from 50g/l to 160g/l, based on the volume of the honeycomb body.
The mass ratio of the carrier material to the oxygen storage component in the coating is generally preferably from 0.2 to 1.5, for example from 0.3 to 0.8.
In an embodiment of the invention, coating a and coating B comprise one or more alkaline earth metal compounds, such as strontium oxide, barium oxide or barium sulfate. The amount of barium sulfate per coating is in particular 2g/l to 20g/l of support volume.
Coating a comprises in particular strontium oxide or barium oxide.
In other embodiments of the invention, coating a and coating B contain additives, such as rare earth compounds, e.g. lanthanum oxide, and/or binders, such as aluminum compounds. The amounts of these additives can vary within wide limits and can be determined in the specific case by a person skilled in the art by simple methods.
Honeycomb bodies made of ceramic or metal, which have a volume V and parallel flow channels for the exhaust gases of internal combustion engines, are suitable as catalytically inert catalyst supports. According to the invention, a catalytically active coating is located on the walls in the channels of the flow substrate. Ceramic honeycombs that can be used in accordance with the invention are known flow substrates and are commercially available. They consist, for example, of silicon carbide, aluminum titanate, or cordierite, and have, for example, a cell density of 200 to 900 cells per square inch (cpsi), and typically a wall thickness of 2 to 12 mils or 0.051 to 0.305 mm. Honeycombs that can be used according to the invention are known and commercially available.
In accordance with the present invention, the coating extends from one end of the ceramic honeycomb body at least 50% beyond the length L of the substrate, the loading of the substrate with the catalytic coating is in total 100g/l to 350g/l, preferably 125g/l to 300g/l, and particularly preferably 150g/l to 280g/l, based on the volume of the support.
In an embodiment of the invention, coating a and coating B are free of zeolites and molecular sieves.
In another embodiment of the invention, layer a is located directly on the inert catalyst support, i.e. there is no additional or internal coating layer between the inert catalyst support and layer a.
In another embodiment of the invention, layer B is in direct contact with the exhaust gas stream, i.e. no additional or internal coating layer is present on layer B.
The catalytic converter according to the invention can be produced by methods known to the person skilled in the art, for example by applying a coating suspension (often referred to as washcoat) to the honeycomb body by one of the customary dip coating methods, or pumps, and suction coating methods. Thermal post-treatment or calcination is usually followed.
According to the present invention, the wall surfaces of the flow channels of the substrate are coated with two catalyst layers a and B. To coat the catalyst support with layer a, the solids provided for this layer are suspended in water and the catalyst support is coated with the coating suspension thus obtained. The process is repeated with the coating suspension, wherein the solids provided for layer B are suspended in water.
Preferably, the layers a and B are coated along the entire length of the inert catalyst support. This means that layer B completely covers layer a, so that only layer B is in direct contact with the exhaust gas flow.
It is known to those skilled in the art that the average particle size of the catalytically active material must be matched to the particular ceramic substrate. In an embodiment of the invention, the coating suspension used to produce the coating is ground to d502 to 8 μm, preferably 3 to 7 μm, particularly preferably 4 to 6 μm, and d90A particle size distribution of 7 to 25 μm, preferably 8 to 23 μm, particularly preferably 9 to 20 μm (mean particle size d of the Q3 distribution according to DIN 66160, latest edition of the filing date, respectively50And d90[https://de.wikipedia.org/wiki/Partikelgr％C3％B6％C3％9Fenverteilung])。
The catalytic converter according to the invention is well suited for removing carbon monoxide, hydrocarbons and nitrogen oxides from the exhaust gases of internal combustion engines operating with a stoichiometric air-fuel mixture, in particular in vehicles with intake manifold injection.
The invention therefore also relates to a method for removing carbon monoxide, hydrocarbons and nitrogen oxides from the exhaust gas of an internal combustion engine which is operated with a stoichiometric air-fuel mixture, characterized in that the exhaust gas is passed through a catalytic converter according to the invention.

Claims (17)

1. Catalytic converter for removing carbon monoxide, hydrocarbons and nitrogen oxides from the exhaust gases of an internal combustion engine operating with a stoichiometric air-fuel mixture, comprising a ceramic flow substrate of length L and at least two catalytic coatings a and B, wherein
Layer A comprises at least one activated alumina, one platinum group metal and at least two different cerium/zirconium/rare earth metal mixed oxides, and
-layer B applied on said layer a comprises at least one activated alumina, one platinum group metal and at least one cerium/zirconium/rare earth metal mixed oxide.
2. The catalytic converter according to claim 1,
it is characterized in that the preparation method is characterized in that,
the coating a is located on the wall of the substrate and extends from one end of the substrate over at least 50% of the length L.
3. Catalytic converter according to claim 1 and/or 2,
it is characterized in that the preparation method is characterized in that,
the weight ratio of the alumina in coating a to the sum of the two cerium/zirconium/rare earth metal mixed oxides is in the range of 10:90 to 60: 40.
4. The catalytic converter according to any one of claims 1 to 3,
it is characterized in that the preparation method is characterized in that,
the weight ratio of the first cerium/zirconium/rare earth metal mixed oxide to the second cerium/zirconium/rare earth metal mixed oxide in coating a is in the range of 4:1 to 1: 4.
5. The catalytic converter of any one of the preceding claims,
it is characterized in that the preparation method is characterized in that,
the first cerium/zirconium/rare earth metal mixed oxide in coating a has a higher zirconia content than the second cerium/zirconium/rare earth metal mixed oxide.
6. The catalytic converter of any one of the preceding claims,
it is characterized in that the preparation method is characterized in that,
the first cerium/zirconium/rare earth metal mixed oxide in coating a has a cerium oxide to zirconium oxide weight ratio of 0.7 to 0.1 that is less than the second cerium/zirconium/rare earth metal mixed oxide in coating a has a cerium oxide to zirconium oxide weight ratio of 0.5 to 1.5.
7. The catalytic converter of any one of the preceding claims,
it is characterized in that the preparation method is characterized in that,
the first cerium/zirconium/rare earth metal mixed oxide in coating a has a cerium oxide content of 10% to 40% based on the weight of the first cerium/zirconium/rare earth metal mixed oxide.
8. The catalytic converter of any one of the preceding claims,
it is characterized in that the preparation method is characterized in that,
the first cerium/zirconium/rare earth metal mixed oxide in coating a has a zirconia content of 40% to 90% based on the weight of the first cerium/zirconium/rare earth metal mixed oxide.
9. The catalytic converter of any one of the preceding claims,
it is characterized in that the preparation method is characterized in that,
the second cerium/zirconium/rare earth metal mixed oxide in coating a has a cerium oxide content of 25% to 60% based on the weight of the second cerium/zirconium/rare earth metal mixed oxide.
10. The catalytic converter of any one of the preceding claims,
it is characterized in that the preparation method is characterized in that,
the second cerium/zirconium/rare earth metal mixed oxide in coating a has a zirconium oxide content of 20% to 70% based on the weight of the second cerium/zirconium/rare earth metal mixed oxide.
11. The catalytic converter of any one of the preceding claims,
it is characterized in that the preparation method is characterized in that,
the two cerium/zirconium/rare earth metal mixed oxides in coating a are both doped with lanthanum oxide.
12. The catalytic converter of any one of the preceding claims,
it is characterized in that the preparation method is characterized in that,
the lanthanum oxide content is > 0% to 10% based on the weight of the corresponding cerium/zirconium/rare earth metal mixed oxide.
13. The catalytic converter of any one of the preceding claims,
it is characterized in that the preparation method is characterized in that,
the first cerium/zirconium/rare earth metal mixed oxide in coating a is doped with yttrium oxide in addition to lanthanum oxide.
14. The catalytic converter of any one of the preceding claims,
it is characterized in that the preparation method is characterized in that,
the second cerium/zirconium/rare earth mixed oxide in coating a is doped not only with lanthanum oxide but also with other metal oxides from the group of rare earth oxides, preferably with praseodymium.
15. The catalytic converter of any one of the preceding claims,
it is characterized in that the preparation method is characterized in that,
the cerium/zirconium/rare earth metal mixed oxide in coating B is doped with yttrium oxide and/or praseodymium oxide in addition to lanthanum oxide.
16. The catalytic converter of any one of the preceding claims,
it is characterized in that the preparation method is characterized in that,
the catalytically active coating comprises the noble metals platinum, palladium, rhodium or mixtures thereof.
17. A method for removing carbon monoxide, hydrocarbons and nitrogen oxides from the exhaust gas of an internal combustion engine operated with a stoichiometric air-fuel mixture,
it is characterized in that the preparation method is characterized in that,
the exhaust gas is conducted through the catalytic converter according to claims 1 to 16.
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